EP0946790B1 - Elektrolyseapparat zur herstellung von halogengasen - Google Patents

Elektrolyseapparat zur herstellung von halogengasen Download PDF

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Publication number
EP0946790B1
EP0946790B1 EP97937576A EP97937576A EP0946790B1 EP 0946790 B1 EP0946790 B1 EP 0946790B1 EP 97937576 A EP97937576 A EP 97937576A EP 97937576 A EP97937576 A EP 97937576A EP 0946790 B1 EP0946790 B1 EP 0946790B1
Authority
EP
European Patent Office
Prior art keywords
electrolysis
anode
cathode
rear wall
housing
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
EP97937576A
Other languages
German (de)
English (en)
French (fr)
Other versions
EP0946790A1 (de
Inventor
Thomas Borucinski
Karl-Heinz Dulle
Jürgen Gegner
Martin Wollny
Helmut Dr. Lademann
Luciano Mose
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
ThyssenKrupp Industrial Solutions AG
Original Assignee
Krupp Uhde GmbH
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Krupp Uhde GmbH filed Critical Krupp Uhde GmbH
Publication of EP0946790A1 publication Critical patent/EP0946790A1/de
Application granted granted Critical
Publication of EP0946790B1 publication Critical patent/EP0946790B1/de
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/60—Constructional parts of cells
    • C25B9/65—Means for supplying current; Electrode connections; Electric inter-cell connections
    • C25B9/66—Electric inter-cell connections including jumper switches
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
    • C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/70—Assemblies comprising two or more cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T29/00—Metal working
    • Y10T29/49—Method of mechanical manufacture
    • Y10T29/49002—Electrical device making

Definitions

  • the invention relates to an electrolysis apparatus for production of halogen gases from aqueous alkali halide solution with several arranged side by side in a stack and plate-shaped electrolytic cells in electrical contact, each made up of two half-shells electrically conductive material with outside contact strips have on at least one rear wall, wherein the housing means for supplying the electrolysis current and electrolysis input materials and facilities for discharging the electrolysis current and the electrolysis products and a substantially planar anode and cathode has, wherein the anode and the cathode by a Partition separated and arranged parallel to each other are and by means of metallic stiffeners with the each assigned rear wall of the housing electrically conductive are connected, the metallic stiffeners as webs aligned with the contact strips are, the side edges over the height of the rear wall and the Anode or cathode on the rear wall and the anode or cathode issue.
  • the invention further relates to a method of manufacture of electrolysis cells for an electrolysis apparatus of the above Type in which the respective housing from each two half shells with the interposition of the required Facilities and the cathode and anode as well as the partition by fixing them by means of webs metallic stiffeners and the anode and Housing or cathode and housing electrically conductive to each other be attached.
  • An electrolysis apparatus is known from EP 0 189 535 B1, at the the anode or the cathode with the respective rear wall the housing halves via truss-like metallic stiffeners connected is.
  • On the back of the anode or Half of the cathode is a contact strip for each electrical contact to the neighboring, identical structure Electrolysis cell attached. The current flows through the contact strip through the back wall into the half-timbered metallic stiffeners and from there it spreads starting from the metallic contact points - stiffening / anode - via the anode.
  • the flow through the Membrane After the flow through the Membrane has passed through, it is taken up by the cathode, to find out about the framework-like stiffeners in the Back wall to flow on the cathode side and then back in the contact strip and from there to the next electrolytic cell to enter.
  • the connection of the current-carrying components is done by spot welding. In the The electrolysis current bundles welding spots to form peak current densities.
  • Another disadvantage of the known electrolysis apparatus is that the framework-like stiffeners that the Connect the back wall and the electrodes together Flexibility reasons not perpendicular between the rear wall and Are arranged, resulting in an extension of the Leads to current paths, which also results in an increase in cell voltage results.
  • the current comes from the framework-like Stiffening in the electrode only selectively, which on the one hand has an uneven power distribution and on the other hand in turn leads to an increase in cell voltage.
  • the uneven current distribution on the electrodes leads moreover to a non-uniform depletion of electrolytes, resulting in a reduction in electricity yield and results in a reduction in membrane life.
  • the object of the invention is to provide an electrolysis apparatus create, in which the current-carrying areas as possible are large in order to provide only a selective introduction into the electrodes and the contact strips and thus an uneven current distribution to avoid.
  • the webs over their entire Height electrically connected to the anode or cathode are.
  • the cathodes can be made of iron, cobalt, nickel or chrome or one of their alloys and the anodes made of titanium, niobium or tantalum or an alloy of these metals or from consist of a metal or oxide ceramic material.
  • the electrodes are preferably catalytic effective coating.
  • the electrodes preferably provided with perforations (perforated sheet, Expanded metal, wattle or thin sheets with blind-like Breakthroughs), so that due to their arrangement in the electrolysis cell, the gases formed during electrolysis easily can enter the back of the electrolytic cell. By this gas discharge is achieved that the electrolyte between the electrodes have the lowest possible gas bubble content and thus has maximum conductivity.
  • the partition is preferably an ion exchange membrane, generally from a copolymer of polytetrafluoroethylene or one of its derivatives and a perfluorovinyl ether sulfonic acid and / or perfluorovinyl carboxylic acid. She cares to ensure that the electrolysis products do not mix and because of their selective permeability for Alkali metal ions the current flow. Also come as a partition also diaphragms in question. A diaphragm is one fine-porous partition that prevents the gases from mixing and an electrolytic connection between cathodes and Represents anode space and thus allows current flow.
  • the webs forming the metallic stiffeners can be formed over the entire surface or with openings or Slots.
  • an inlet distributor is provided via which the electrolytes can be fed into the half-shells are.
  • This inlet distributor is preferably like this designed that each segment of a half-shell over at least an opening in the inlet manifold with fresh electrolyte can be supplied and the sum of the areas of the openings in the inlet manifold less than or equal to the cross-sectional area of the inlet distributor.
  • the anode half-shells preferably consist of a counter Halogens and saline resistant material while the cathode half-shells preferably from one against alkali eyes resistant material.
  • a generic method for producing the above Electrolysis apparatus is distinguished according to the invention characterized in that the metallic, electrically conductive Connection of the stiffeners designed as webs with the respective rear wall and the respective contact strip as well the anode or cathode using a reductive sintering process or is produced using a welding process.
  • an adhesive consisting essentially of an oxidic material, for example NiO, and an organic binder is used. This adhesive is spread on the web and the component to be connected to it, for example the rear wall, and the two parts are pressed together using a holding device. After the organic binder has hardened, the oxidic component of the adhesive is reductively sintered in a reducing atmosphere (eg H 2 , CO, etc.).
  • a reducing atmosphere eg H 2 , CO, etc.
  • a welding process is used, a is preferred Laser beam welding process used. It becomes special preferably the laser beam is perpendicular to the welding direction polarized to a significantly reduced ratio to reach from the upper track width to the connection width.
  • the laser beam can preferably be by means of mirror optics be shaped so that by means of a special beam shaping two or more at a time selectable Amount of offset focus points are generated.
  • the laser beam by means of a high-frequency scanner drive, preferably a piezo quartz, by a selectable amount is scanned across the welding direction.
  • a generally designated 1 electrolysis apparatus for Production of halogen gases from aqueous alkali halide solution has several, side by side in a stack arranged and in electrical contact plate-shaped Electrolysis cells 2, of which in Figure 1 exemplary two such electrolysis cells 2 side by side are shown arranged.
  • Each of these electrolytic cells 2 has a housing made of two half-shells 3, 4, which are provided with flange-like edges, between which by means of seals 5 each have a partition (membrane) 6 is clamped. Clamping the membrane 6 can be done in another way if necessary.
  • each on the membrane 6 is adjacent to a flat anode 8 and a flat cathode 9 is provided, the anode 8 or the cathode 9 in each case in alignment with the contact strips 7 arranged stiffeners are connected, the are designed as webs 10.
  • the webs are 10 preferably along its entire side edge 10A the anode or cathode 8, 9 is attached in a metallically conductive manner.
  • To feed and discharge the electrolysis input materials to allow the electrolysis products to rejuvenate the webs 10 starting from the side edges 10A, across its width to the adjacent side edge 10B and have a height there that corresponds to the height of the contact strips 7 corresponds. Accordingly, they are with their margins 10B over the entire height of the contact strips 7 on the rear sides opposite the contact strips 7 the rear walls 3A and 4A attached.
  • a suitable one is to supply the electrolysis products Device provided for the respective electrolysis cell 2, such a device is indicated by 11. There is also a device in every electrolysis cell provided for removing the electrolysis products, these is not indicated, however.
  • the electrodes (anode 8 and cathode 9) are designed such that they are the electrolysis input product or the Flow through raw materials or let them flow freely, for which purpose corresponding slots 8A or the like are provided are, as can also be seen in Fig. 2.
  • the Stringing together several plate-shaped electroyse cells 2 happens in a framework, the so-called cell framework.
  • the plate-shaped electrolytic cells are between the two upper side members of the cell frame suspended in such a way that their plate plane is perpendicular to the longitudinal beam axis stands. So that the plate-shaped electrolysis cells 2 their weight on the upper flange of the side member can transfer, they have on the upper plate edge a cantilever-like holder on each side.
  • the holder extends horizontally in the direction of the Plate level and protrudes over the edges of the flanges out. With the plate-shaped ones suspended in the scaffold Electrolysis cells lie the lower edge of the cantilever-like Holder on the upper flange.
  • the plate-shaped electrolysis cells 2 hang comparatively like folders in a hanging file in the cell structure.
  • the plate surfaces of the electrolysis cells are in the cell frame in mechanical and electrical contact, as if they were stacked. Electrolysers this Design are called electrolysers in a hanging stack type.
  • electrolytic cells 2 By lining up several electrolytic cells 2 in a hanging stack design using known tensioning devices become the electrolytic cells 2 over the contact strips 7 each with adjacent electrolytic cells in one Stack electrically connected. From the contact strips 7 the current then flows through the half-shells over the webs 10 into the anode 8. After passing through the membrane 6 the current is absorbed by the cathode 9, to cross over the webs 10 into the other half-shell or the back wall 3A to flow and here in the contact strip 7 to cross the next cell. In this manner and way the electrolysis current passes through the whole Electrolysis cell stack, being on the one outer cell initiated and derived on the other outer cell becomes.
  • Electrolysis cell is a section of a rear wall of the housing 4A of the half-shell 4, on which a U-shaped contact strip 7 is attached. It is good too recognize that on the back aligned with the contact strip 7 is attached to the rear wall 4A a web 10 is, the web 10 is approximately in the center of the U-shaped profiled contact strip 7, which is related 4A to 4C explained in more detail below becomes. On the other side edge 10A of the web 10 this attached to the anode 8, which in the area of Connection with the webs 10 is formed over the entire surface, while adjacent to these areas to pass through Electrolysis input and output products slots 8A are provided. The connection is the same between the respective web 10 and the cathode 9 educated.
  • the Web 10 have a different design.
  • the webs 10 are full-surface formed, only the two side edges 10A and 10B different for the reasons mentioned above are long.
  • the webs 10 Open slots 13.
  • the embodiment according to Figure 3D, in which the web 10 is shown in a side view according to FIG. 3C is also has slots, which from angled Die cuts 15 are formed.
  • the webs 10 have a maximum cross-sectional area for the Current flow provided because of this in principle along its entire length with both the rear wall of the housing 3A or 4A as well as with the respective electrode 8 or 9 is metallically connected.
  • the current path is minimized, since the web 10 is the vertical connection between the housing rear wall 3A or 4A and the electrode 8 or 9 represents.
  • connection of the web 10 to the electrode 8 or 9 or with the rear wall 3A or 4A is preferred designed in such a way that no joining surfaces are created, the additional Surface contact resistors for current flow would form. It is therefore preferred between the a metallic double or Triple composite manufactured, preferably by a laser beam welding process, although basically also conventional Welding processes, e.g. Resistance welding, can be used. Beyond that too reductive sintering process possible.
  • the welded joint can possibly, in order to minimize the welding process To ensure heat input and thus minimal warpage, also done selectively.
  • There is also a welded joint possible over the entire individual cell height whereby a continuous connection is preferable because therefore an optimal current distribution, minimal contact resistance and thus a minimum possible cell voltage is achieved.
  • FIGS. 4A to 4C Different embodiments of a triple composite in Laser welding processes are shown in FIGS. 4A to 4C, in each of which a contact strip 7, a Part of a rear wall 4A and the side edge 10B of a web are shown.
  • the weld seam 16 which is produced forms a pronounced one Chalice shape.
  • a typical relationship results from top track width to connection width of 2.5.
  • a seam shape was used with the same laser beam source and focusing optics as in the embodiment of Figure 4A, but using one polarized perpendicular to the welding direction Laser beam reached, so that as a result of the seam flanks acting increased beam coupling through the Brewster effect resulted in a significant widening of the seam is.
  • This seam is labeled 16 ''.
  • the ratio of the upper track width to the connection width at about 1.6.
  • the seam volume was in this case in the same order of magnitude as for welding Figure 4A, but the port width is almost 25% elevated.
  • a particularly good ratio of top track width the welded joint shows the connection width of 1.5 according to Figure 4C, which is designated there with 16 '' '.
  • the connection width is 50% higher than with the welded connection according to FIG. 4A.
  • the one shown here Seam shape 16 '' ' was created using a special Beam shaping with the same laser beam source as in of the welded connection according to FIG. 4B.
  • the laser beam with special mirror optics shaped so that two were offset by about 0.5 mm at the same time Focus points were created.
  • Such a seam shape can also be done by high-frequency scanning of the focusing mirror with an amplitude of e.g. 0.5 mm realized become.
  • the figures are not shown in detail Design of the electrolysis cells 2 in the lower area with the electrolyte entry.
  • the electrolyte entry can both selectively and with a so-called inlet distributor respectively.
  • the inlet distributor is designed so that a tube is arranged in the element that over Openings. Since a half-shell through the webs 10, the connection between the rear walls 3A and 4A and represent the electrodes 8, 9, is segmented you get an optimal concentration distribution if both Half-shells 3, 4 equipped with an inlet distributor are, the length of which is arranged in the half-shell Inlet distributor corresponds to the width of the half-shell and each segment through at least one opening in the inlet manifold supplied with the respective electrolyte becomes.
  • the sum of the cross-sectional area of the openings in the Inlet manifold should be smaller than or equal to that Inner pipe cross section of the distributor pipe.
  • the two half-shells 3, 4 provided with flanges in the flange area, that are screwed.
  • the cells thus constructed are in a cell structure, not shown, is either attached or posed. Hooking or placing in the cell structure takes place on the flanges, not shown holding devices located.
  • the electrolysis machine 1 may consist of a single cell, or preferably by stringing together several electrolysis cells 2 in hanging stack design. Become several single cells pressed together according to the hanging stack principle the individual cells are aligned plane-parallel before the clamping device is closed, otherwise the No current transfer from one single cell to the next can take place over all contact strips 7.
  • the brackets or not shown contact surfaces on the cell frame and cell frame provided with assigned coatings.
  • a plastic e.g. PE, PP, PVC, PFA, FEP, E / TFE, PVDF or PTFE relined, while the contact surfaces on Cell structure also coated with one of these plastics is.
  • the plastic can only be put on and guided over a groove, glued, welded or be screwed on. It is only essential that the Plastic pad is fixed.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
EP97937576A 1996-10-05 1997-08-13 Elektrolyseapparat zur herstellung von halogengasen Expired - Lifetime EP0946790B1 (de)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE19641125 1996-10-05
DE19641125A DE19641125A1 (de) 1996-10-05 1996-10-05 Elektrolyseapparat zur Herstellung von Halogengasen
PCT/EP1997/004402 WO1998015675A1 (de) 1996-10-05 1997-08-13 Elektrolyseapparat zur herstellung von halogengasen

Publications (2)

Publication Number Publication Date
EP0946790A1 EP0946790A1 (de) 1999-10-06
EP0946790B1 true EP0946790B1 (de) 2001-10-17

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EP97937576A Expired - Lifetime EP0946790B1 (de) 1996-10-05 1997-08-13 Elektrolyseapparat zur herstellung von halogengasen

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US (1) US6282774B1 (nl)
EP (1) EP0946790B1 (nl)
JP (1) JP4086321B2 (nl)
KR (1) KR100496750B1 (nl)
CN (1) CN1174120C (nl)
AR (1) AR008492A1 (nl)
AT (1) ATE207140T1 (nl)
AU (1) AU721458B2 (nl)
BR (1) BR9712266A (nl)
CA (1) CA2265738C (nl)
CZ (1) CZ83999A3 (nl)
DE (2) DE19641125A1 (nl)
HU (1) HUP9903787A2 (nl)
ID (1) ID18532A (nl)
IL (1) IL129245A (nl)
IN (1) IN192330B (nl)
JO (1) JO1983B1 (nl)
MA (1) MA24362A1 (nl)
MY (1) MY117917A (nl)
NO (1) NO319567B1 (nl)
PL (1) PL188243B1 (nl)
RO (1) RO119632B1 (nl)
RU (1) RU2176289C2 (nl)
SK (1) SK35999A3 (nl)
TR (1) TR199900616T2 (nl)
WO (1) WO1998015675A1 (nl)
ZA (1) ZA978862B (nl)

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DE10249508A1 (de) 2002-10-23 2004-05-06 Uhde Gmbh Elektrolysezelle mit Innenrinne
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DE102006020374A1 (de) * 2006-04-28 2007-10-31 Uhdenora S.P.A. Mikrostrukturierter Isolierrahmen für Elektrolysezellen
DE102006028168A1 (de) * 2006-06-16 2007-12-20 Uhde Gmbh Vorrichtung zur elektrochemischen Wasseraufbereitung
DE102006057386A1 (de) * 2006-12-04 2008-06-05 Uhde Gmbh Verfahren zum Beschichten von Substraten
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IT1391774B1 (it) * 2008-11-17 2012-01-27 Uhdenora Spa Cella elementare e relativo elettrolizzatore modulare per processi elettrolitici
DE102010023410A1 (de) 2010-06-11 2011-12-15 Uhde Gmbh Verwendung einer Platinelektrode zur Persulfatelektrolyse
DE102010023418A1 (de) 2010-06-11 2011-12-15 Uhde Gmbh Ein- oder mehrseitige Substratbeschichtung
DE102010054643A1 (de) 2010-12-15 2012-06-21 Bayer Material Science Ag Elektrolyseur mit spiralförmigem Einlaufschlauch
DE102011117454B4 (de) * 2011-10-31 2021-11-25 Precitec Gmbh & Co. Kg Laserbearbeitungsvorrichtung
DE102012015802A1 (de) 2012-08-10 2014-02-13 Thyssenkrupp Uhde Gmbh Verfahren zur Herstellung von Elektrolysezellen-Kontaktstreifen
DE102012017306A1 (de) 2012-09-03 2014-03-06 Thyssenkrupp Uhde Gmbh Elektrochemische Zelle vom Durchflusstyp
US8808512B2 (en) 2013-01-22 2014-08-19 GTA, Inc. Electrolyzer apparatus and method of making it
JP6028007B2 (ja) * 2014-10-24 2016-11-16 株式会社イープラン 電解槽の製作方法
US10407783B2 (en) 2016-05-26 2019-09-10 Calera Corporation Anode assembly, contact strips, electrochemical cell, and methods to use and manufacture thereof
DE102017217364B4 (de) 2017-09-29 2019-08-22 Thyssenkrupp Uhde Chlorine Engineers Gmbh Elektrolysezelle mit Vorspannkupplung, Verfahren zum Montieren der Vorspannkupplung sowie Verwendung der Vorspannkupplung
EP4053307A1 (en) 2021-03-01 2022-09-07 thyssenkrupp nucera AG & Co. KGaA Electrolysis cell, electrolysis device for chlor-alkali electrolysis and use of an electrolysis cell for chlor-alkali electrolysis
WO2022258394A1 (en) 2021-06-07 2022-12-15 thyssenkrupp nucera AG & Co. KGaA Electrolysis cell and electrolyzer
AU2022308316A1 (en) 2021-07-08 2023-12-14 thyssenkrupp nucera AG & Co. KGaA Electrolyzer with multi-cell elements
EP4123057A1 (de) 2021-07-19 2023-01-25 Covestro Deutschland AG Optimierter flüssigkeitsablauf aus membranelektrolyseuren
EP4194587B1 (en) 2021-12-08 2024-06-26 thyssenkrupp nucera AG & Co. KGaA Electrolyzer with a cell casing made from metal foil
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Also Published As

Publication number Publication date
CA2265738C (en) 2011-01-25
DE19641125A1 (de) 1998-04-16
DE59705007D1 (de) 2001-11-22
AR008492A1 (es) 2000-01-19
CN1174120C (zh) 2004-11-03
IL129245A (en) 2001-12-23
PL332512A1 (en) 1999-09-13
JP2001506314A (ja) 2001-05-15
IN192330B (nl) 2004-04-10
NO991461D0 (no) 1999-03-25
EP0946790A1 (de) 1999-10-06
US6282774B1 (en) 2001-09-04
IL129245A0 (en) 2000-02-17
MY117917A (en) 2004-08-30
SK35999A3 (en) 1999-07-12
AU721458B2 (en) 2000-07-06
AU4015197A (en) 1998-05-05
NO991461L (no) 1999-03-25
RO119632B1 (ro) 2005-01-28
NO319567B1 (no) 2005-08-29
PL188243B1 (pl) 2005-01-31
ZA978862B (en) 1999-04-06
JO1983B1 (en) 1997-12-15
BR9712266A (pt) 1999-08-24
CA2265738A1 (en) 1998-04-16
WO1998015675A1 (de) 1998-04-16
KR100496750B1 (ko) 2005-06-22
TR199900616T2 (xx) 1999-06-21
CZ83999A3 (cs) 1999-10-13
JP4086321B2 (ja) 2008-05-14
HUP9903787A2 (hu) 2000-04-28
ATE207140T1 (de) 2001-11-15
KR20000048491A (ko) 2000-07-25
CN1232512A (zh) 1999-10-20
RU2176289C2 (ru) 2001-11-27
ID18532A (id) 1998-04-16
MA24362A1 (fr) 1998-07-01

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